Unveiling the Stability of Encapsulated Pt Catalysts Using Nanocrystals and Atomic Layer Deposition

被引:5
|
作者
Liccardo, Gennaro [1 ,2 ,3 ]
Cendejas, Melissa C. [4 ]
Mandal, Shyama C. [1 ,2 ,3 ]
Stone, Michael L. [1 ,2 ]
Porter, Stephen [5 ]
Nhan, Bang T. [6 ]
Kumar, Abinash [7 ]
Smith, Jacob [7 ,8 ]
Plessow, Philipp N. [9 ]
Cegelski, Lynette [6 ]
Osio-Norgaard, Jorge [1 ,2 ]
Abild-Pedersen, Frank [3 ]
Chi, Miaofang [7 ,10 ]
Datye, Abhaya K. [5 ]
Bent, Stacey F. [1 ,2 ,11 ]
Cargnello, Matteo [1 ,2 ,3 ]
机构
[1] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA
[2] Stanford Univ, SUNCAT Ctr Interface Sci & Catalysis, Stanford, CA 94305 USA
[3] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA
[4] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA
[5] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA
[6] Stanford Univ, Dept Chem, Stanford, CA 94305 USA
[7] Oak Ridge Natl Lab, Oak Ridge, TN 37830 USA
[8] North Carolina State Univ, Dept Mat Sci & Engn, Raleigh, NC 27695 USA
[9] Karlsruhe Inst Technol, Inst Catalysis Res & Technol, D-76344 Eggenstein Leopoldshafen, Germany
[10] Duke Univ, Dept Mech Engn & Mat Sci, Durham, NC 27708 USA
[11] Stanford Univ, Dept Energy Sci & Engn, Stanford, CA 94305 USA
基金
美国国家科学基金会;
关键词
TOTAL-ENERGY CALCULATIONS; WATER-GAS SHIFT; PLATINUM; CERIA; NANOPARTICLES; OXIDATION; TEMPERATURE; PARTICLES; METALS; SITE;
D O I
10.1021/jacs.4c06423
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Platinum exhibits desirable catalytic properties, but it is scarce and expensive. Optimizing its use in key applications such as emission control catalysis is important to reduce our reliance on such a rare element. Supported Pt nanoparticles (NPs) used in emission control systems deactivate over time because of particle growth in sintering processes. In this work, we shed light on the stability against sintering of Pt NPs supported on and encapsulated in Al2O3 using a combination of nanocrystal catalysts and atomic layer deposition (ALD) techniques. We find that small amounts of alumina overlayers created by ALD on preformed Pt NPs can stabilize supported Pt catalysts, significantly reducing deactivation caused by sintering, as previously observed by others. Combining theoretical and experimental insights, we correlate this behavior to the decreased propensity of oxidized Pt species to undergo Ostwald ripening phenomena because of the physical barrier imposed by the alumina overlayers. Furthermore, we find that highly stable catalysts can present an abundance of under-coordinated Pt sites after restructuring of both Pt particles and alumina overlayers at a high temperature (800 degrees C) in C3H6 oxidation conditions. The enhanced stability significantly improves the Pt utilization efficiency after accelerated aging treatments, with encapsulated Pt catalysts reaching reaction rates more than two times greater than those of a control supported Pt catalyst.
引用
收藏
页码:23909 / 23922
页数:14
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